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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Assessing the Importance of the H-2-H2O-H2O Three-Body Interaction on the Vibrational Frequency Shift of H-2 in the sII Clathrate Hydrate and Comparison with Experiment
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Assessing the Importance of the H-2-H2O-H2O Three-Body Interaction on the Vibrational Frequency Shift of H-2 in the sII Clathrate Hydrate and Comparison with Experiment

机译：评估H-2-H2O-H2O三体相互作用对SII Clathrate水合物中H-2振动频率的重要性及与实验比较

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摘要

The vibrational frequency shift of H-2 in the 5(12) cage of the sII clathrate hydrate with and without surrounding water molecules is reported at 0 K, using diffusion Monte Carlo calculations for the ground and first excited vibrational states of H-2. Approximate Id calculations of the frequency shift are also reported with the H-2 at the equilibrium position in the clathrate hydrate. These calculations make use of full-dimensional potential energy surfaces for the H-2-H2O 2-body and H-2-H2O-H2O 3-body interactions. The inclusion of the 3-body interaction is shown to make roughly a 33% contribution to the frequency shift and to bring the calculated value of -40 +/- 4 cm(-1) to within just 3 cm(-1) of the experimental value at 20 K. This level of agreement with experiment may be somewhat fortuitous; however, the importance of the 3-body interaction is firmly established by these calculations. The frequency shift reported here with 2-body interactions does not agree with a previously reported calculation using just 2-body interactions from a different ab initio potential energy surface and with a different method to obtain the frequency shift. A similar Id calculation of the frequency shift using that potential is reported and agrees to within roughly 10% of the one previously reported. Therefore, this suggests that the difference between the present calculations and the previous one using just 2-body interactions is mainly due to differences in the potential energy surfaces.
机译：在0 k下，使用扩散蒙特卡罗计算，在0 k下报道，使用围绕水分子的SiI Clathrate水合物的5（12）个笼子中的H-2的振动频率偏移，其用于地面和首先激发H-2的激发振动状态。 H-2在包裹水合物的平衡位置处的H-2报告了频移的近似ID计算。这些计算利用H-2-H2O 2-mobit和H-2-H 2 O-H2O 3体相互作用的全尺寸势能表面。显示3体相互作用的含量为频移大约为33％的贡献，并将计算值-40 +/- 4 cm（-1）的计算值带到仅3厘米（-1）内20 K的实验值。这种与实验的协议水平可能有些偶然;然而，这些计算牢固建立了3体相互作用的重要性。这里报告的频移具有2体相互作用不一致使用从不同的AB Initio潜在能量表面的2对相互作用以及不同的方法来获得先前报告的计算，以获得频移。报告了使用该电位的频率偏移的类似ID计算，并同意在先前报告的大约10％之内。因此，这表明目前计算与使用仅2体相互作用的差异主要是由于潜在能量表面的差异。

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